Nanomaterials ◽  
2020 ◽  
Vol 10 (11) ◽  
pp. 2246
Author(s):  
Haonan Duan ◽  
Yajie Tian ◽  
Siyuan Gong ◽  
Bofeng Zhang ◽  
Zongjing Lu ◽  
...  

Herein, Pt/HZSM-5 zeolite catalysts with different crystallite sizes ranging from nanosheet (~2 nm) to bulk crystals (~1.5 μm) have been prepared for the hydrodeoxygenation of guaiacol, and their effects on the reaction pathway and product selectivity were explored. HZSM-5 zeolites prepared by seeding (Pt/Z-40: ~40 nm) or templating (Pt/NS-2: ~2 nm) fabricated intra-crystalline mesopores and thus enhanced the reaction rate by promoting the diffusion of various molecules, especially the bulky ones such as guaiacol and 2-methoxycyclohexanol, leading to a higher cyclohexane selectivity of up to 80 wt % (both for Pt/Z-40 and Pt/NS-2) compared to 70 wt % for bulky HZSM-5 (Pt/CZ: ~1.5 μm) at 250 °C and 120 min. Furthermore, decreased crystallite sizes more effectively promoted the dispersion of Pt particles than bulky HZSM-5 (Pt/Z-400: ~400 nm and Pt/CZ). The relatively low distance between Pt and acidic sites on the Pt/Z-40 catalyst enhanced the metal/support interaction and induced the reaction between the guaiacol molecules adsorbed on the acidic sites and the metal-activated hydrogen species, which was found more favorable for deoxygenation than for hydrogenation of oxygen-containing molecules. In addition, Pt/NS-2 catalyst with a highly exposed surface facilitated more diverse reaction pathways such as alkyl transfer and isomerization.


2021 ◽  
Author(s):  
Liang Wei ◽  
Jian Chen ◽  
Shuai Lyu ◽  
Chengchao Liu ◽  
Yanxi Zhao ◽  
...  

The delicate balance between dispersion and reduction of the Co-based Fischer–Tropsch synthesis catalyst is the golden key to enhancing catalytic performance, which highly depends on an optimized metal–support interaction. In...


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Yi Shi ◽  
Zhi-Rui Ma ◽  
Yi-Ying Xiao ◽  
Yun-Chao Yin ◽  
Wen-Mao Huang ◽  
...  

AbstractTuning metal–support interaction has been considered as an effective approach to modulate the electronic structure and catalytic activity of supported metal catalysts. At the atomic level, the understanding of the structure–activity relationship still remains obscure in heterogeneous catalysis, such as the conversion of water (alkaline) or hydronium ions (acid) to hydrogen (hydrogen evolution reaction, HER). Here, we reveal that the fine control over the oxidation states of single-atom Pt catalysts through electronic metal–support interaction significantly modulates the catalytic activities in either acidic or alkaline HER. Combined with detailed spectroscopic and electrochemical characterizations, the structure–activity relationship is established by correlating the acidic/alkaline HER activity with the average oxidation state of single-atom Pt and the Pt–H/Pt–OH interaction. This study sheds light on the atomic-level mechanistic understanding of acidic and alkaline HER, and further provides guidelines for the rational design of high-performance single-atom catalysts.


Nanoscale ◽  
2020 ◽  
Vol 12 (27) ◽  
pp. 14825-14830
Author(s):  
Kai-Qiang Jing ◽  
Yu-Qing Fu ◽  
Zhi-Qiao Wang ◽  
Zhe-Ning Chen ◽  
Hong-Zi Tan ◽  
...  

Zn2+-Modified MgAl-LDH with ultra-low Pd cluster loading was synthesized. The higher adsorption energy and strong covalent metal–support interaction via forming Pd–Zn bonds over Pd/ZnMgAl-LDH account for the robust catalytic performance.


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